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Perrot danced often with the great Romantic ballerina, Marie Taglioni but their partnership was short-lived. She eventually refused to dance with him fearing that he would outshine her.

Perrot left the Opéra in 1835 to tour European dance centers such as London, Milan, Vienna and Naples, where he met and noticed the talent of Carlotta Grisi. He coached her and presented her to the world as the next great ballerina in an 1836 performance in London with himself as her partner.[1] In that same year Perrot began to experiment with the art of choreography.

Following the success of his contributions to the choreography of Giselle, Perrot went on to choreograph Alma ou La Fille du Feu (London 1842) for Fanny Cerrito, which was hailed as a major choreographic success. For the next six years he choreographed regularly at Her Majesty's Theatre in London, including Ondine (1843), La Esmeralda (1844) Le Judgement de Paris (1846) and the famous Pas de Quatre on 12 July 1845. For this ballet he not only negotiated the difficult task of persuading the four leading ballerinas of the day to appear on stage together, but also created a choreographic masterpiece. The event took place at Her Majesty's Theatre in London. Nearly every ballet Perrot ever created was set to the music of Cesare Pugni.

Next, Perrot was engaged as a dancer in St. Petersburg for the Imperial Ballet and later was appointed Balletmaster there. He remained with the Imperial Russian Ballet until 1858. While there, he married Capitoline Samovskaya, a pupil at the Imperial Theater School, with whom he had two children. Uncommitted about whether to remain in Russia or return to Paris, his mind was made up by an incident in his apartment: without any apparent cause, a large mirror fell from the wall and crashed into many small pieces. He returned to Paris to a life of comparative leisure.